Seasonality of the particle number concentration and size distribution: A global analysis retrieved from the network of Global Atmosphere Watch (GAW) near-surface observatories

Clemence Rose, Martine Collaud Coen, Elisabeth Andrews, Yong Lin, Isaline Bossert, Cathrine Lund Myhre, Thomas Tuch, Alfred Wiedensohler, Markus Fiebig, Pasi Aalto, Andres Alastuey, Elisabeth Alonso-Blanco, Marcos Andrade, Begona Artinano, Todor Arsov, Urs Baltensperger, Susanne Bastian, Olaf Bath, Johan Paul Beukes, Benjamin T. BremNicolas Bukowiecki, Juan Andres Casquero-Vera, Sebastien Conil, Konstantinos Eleftheriadis, Olivier Favez, Harald Flentje, Maria I. Gini, Francisco Javier Gomez-Moreno, Martin Gysel-Beer, Anna Gannet Hallar, Ivo Kalapov, Nikos Kalivitis, Anne Kasper-Giebl, Melita Keywood, Jeong Eun Kim, Sang Woo Kim, Adam Kristensson, Markku Kulmala, Heikki Lihavainen, Neng Huei Lin, Hassan Lyamani, Angela Marinoni, Sebastiao Martins Dos Santos, Olga L. Mayol-Bracero, Frank Meinhardt, Maik Merkel, Jean Marc Metzger, Nikolaos Mihalopoulos, Jakub Ondracek, Marco Pandolfi, Noemi Perez, Tuukka Petaja, Jean Eudes Petit, David Picard, Jean Marc Pichon, Veronique Pont, Jean Philippe Putaud, Fabienne Reisen, Karine Sellegri, Sangeeta Sharma, Gerhard Schauer, Patrick Sheridan, James Patrick Sherman, Andreas Schwerin, Ralf Sohmer, Mar Sorribas, Junying Sun, Pierre Tulet, Ville Vakkari, Pieter Gideon Van Zyl, Fernando Velarde, Paolo Villani, Stergios Vratolis, Zdenek Wagner, Sheng Hsiang Wang, Kay Weinhold, Rolf Weller, Margarita Yela, Vladimir Zdimal, Paolo Laj

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Abstract

Aerosol particles are a complex component of the atmospheric system which influence climate directly by interacting with solar radiation, and indirectly by contributing to cloud formation. The variety of their sources, as well as the multiple transformations they may undergo during their transport (including wet and dry deposition), result in significant spatial and temporal variability of their properties. Documenting this variability is essential to provide a proper representation of aerosols and cloud condensation nuclei (CCN) in climate models. Using measurements conducted in 2016 or 2017 at 62 ground-based stations around the world, this study provides the most up-to-date picture of the spatial distribution of particle number concentration (Ntot) and number size distribution (PNSD, from 39 sites). A sensitivity study was first performed to assess the impact of data availability on Ntot's annual and seasonal statistics, as well as on the analysis of its diel cycle. Thresholds of 50g% and 60g% were set at the seasonal and annual scale, respectively, for the study of the corresponding statistics, and a slightly higher coverage (75g%) was required to document the diel cycle. Although some observations are common to a majority of sites, the variety of environments characterizing these stations made it possible to highlight contrasting findings, which, among other factors, seem to be significantly related to the level of anthropogenic influence. The concentrations measured at polar sites are the lowest (g1/4g102gcm-3) and show a clear seasonality, which is also visible in the shape of the PNSD, while diel cycles are in general less evident, due notably to the absence of a regular day-night cycle in some seasons. In contrast, the concentrations characteristic of urban environments are the highest (g1/4g103-104gcm-3) and do not show pronounced seasonal variations, whereas diel cycles tend to be very regular over the year at these stations. The remaining sites, including mountain and non-urban continental and coastal stations, do not exhibit as obvious common behaviour as polar and urban sites and display, on average, intermediate Ntot (g1/4g102-103gcm-3). Particle concentrations measured at mountain sites, however, are generally lower compared to nearby lowland sites, and tend to exhibit somewhat more pronounced seasonal variations as a likely result of the strong impact of the atmospheric boundary layer (ABL) influence in connection with the topography of the sites. ABL dynamics also likely contribute to the diel cycle of Ntot observed at these stations. Based on available PNSD measurements, CCN-sized particles (considered here as either >50gnm or >100gnm) can represent from a few percent to almost all of Ntot, corresponding to seasonal medians on the order of g1/4g10 to 1000gcm-3, with seasonal patterns and a hierarchy of the site types broadly similar to those observed for Ntot. Overall, this work illustrates the importance of in situ measurements, in particular for the study of aerosol physical properties, and thus strongly supports the development of a broad global network of near surface observatories to increase and homogenize the spatial coverage of the measurements, and guarantee as well data availability and quality. The results of this study also provide a valuable, freely available and easy to use support for model comparison and validation, with the ultimate goal of contributing to improvement of the representation of aerosol-cloud interactions in models, and, therefore, of the evaluation of the impact of aerosol particles on climate.

Original languageEnglish
Pages (from-to)17185-17223
Number of pages39
JournalAtmospheric Chemistry and Physics
Volume21
Issue number22
DOIs
StatePublished - 25 Nov 2021

Bibliographical note

Funding Information:
Acknowledgements. NOAA base funding supports the observatories BRW, BND, MLO, SMO, SPO and THD, where efforts of the dedicated observatory staff and of programmer Derek Hageman are appreciated. BRW observations are also supported in part by the Atmospheric Radiation Measurement (ARM) user facility, a US Department of Energy (DOE) Office of Science user facility managed by the Biological and Environmental Research programme.

Funding Information:
Pallas and SMEAR II are grateful for the support of the Academy of Finland Centre of Excellence programme (project no. 272041), the Academy of Finland project Greenhouse gas, aerosol and albedo variations in the changing Arctic (project no. 269095), and the Novel Assessment of Black Carbon in the Eurasian Arctic: From Historical Concentrations and Sources to Future Climate Impacts (NABCEA, project no. 296302).

Funding Information:
CPC measurements at Sonnblick are supported by the Climate and Air Quality Commission of the Austrian Academy of Sciences and the office of the provincial government Salzburg, Unit 5/02.

Funding Information:
Measurements at the Madrid site were funded by the following projects: CRISOL (CGL2017–85344-R MINECO/AEI/FEDER, UE), TIGAS-CM (Madrid Regional Government Y2018/EMT5177), AIRTEC-CM (Madrid Regional Government P2018/EMT4329), REDMAAS2020 (RED2018-102594-T CIENCIA) and Red de Excelencia ACTRIS-ESPAÑA (CGL2017-90884-REDT). Measurements at Montsec and Montseny were supported by the Spanish Ministry of Economy, Industry and Competitiveness and FEDER funds under project HOUSE (CGL2016-78594-R) and by the Generalitat de Catalunya (AGAUR 2017 SGR41 and the DGQA). Aerosol measurements at El Arenosillo Observatory are supported by the National Institute for Aerospace Technology and by different R&D projects of the Ministerio Español de Economía, Industria y Competitivi-dad (MINECO). Aerosol measurements at UGR are supported by the Spanish Ministry of Economy and Competitiveness through projects no. CGL2016-81092-R, CGL2017-90884-REDT, RTI2018-097864-B-I00 and PGC2018-098770-B-I00 and by the Andalusia Regional Government through project no. P18-RT-3820.

Funding Information:
Aerosol measurements at Anmyeon-do were supported by the Korea Meteorological Administration Research and Development Program “Development of Monitoring and Analysis Techniques for Atmospheric Composition in Korea” under grant KMA2018-00522. Measurements at Gosan were supported by the National Research Foundation of Korea (2017R1D1A1B06032548) and the Korea Meteorological Administration Research and Development Program under grant KMI2018-01111.

Funding Information:
The Lulin station is operated under the grants funded by the Taiwan Environmental Protection Administration.

Funding Information:
1Université Clermont Auvergne, CNRS, Laboratoire de Météorologie Physique (LaMP), 63000 Clermont-Ferrand, France 2Federal Office of Meteorology and Climatology, MeteoSwiss, Payerne, Switzerland 3Cooperative Institute for Research in Environmental Sciences, University of Colorado, Boulder, CO, USA 4NOAA Global Monitoring Laboratory, Boulder, CO, USA 5Dept. Atmospheric and Climate Research, NILU-Norwegian Institute for Air Research, Kjeller, Norway 6Physics department, Université Bourgogne Franche Comté, Besançon, France 7Experimental Aerosol and Cloud Microphysics, Leibniz Institute for Tropospheric Research, Leipzig, Germany 8Institute for Atmospheric and Earth System Research, University of Helsinki, Helsinki, Finland 9Institute of Environmental Assessment and Water Research (IDAEA), Spanish Research Council (CSIC), Barcelona, Spain 10Center for Energy, Environmental and Technological Research (CIEMAT), Madrid, Spain 11Laboratorio de Fisica de la Atmosfera, Universidad Mayor de San Andres, La Paz, Bolivia 12Institute for Nuclear Research and Nuclear Energy, Bulgarian Academy of Sciences, Sofia, Bulgaria 13Laboratory of Atmospheric Chemistry, Paul Scherrer Institute, Villigen PSI, Switzerland 14Saxon State Office for Environment, Agriculture and Geology (LfULG), Dresden, Germany 15German Environment Agency (UBA), Zugspitze, Germany 16Atmospheric Chemistry Research Group, Chemical Resource Beneficiation, North-West University, Potchefstroom, 2520, South Africa 17Department of Applied Physics, University of Granada, Granada, Spain 18Andalusian Institute for Earth System Research (IISTA-CEAMA), University of Granada, Autonomous Government of Andalusia, Granada, Spain 19ANDRA DRD/GES Observatoire Pérenne de l’Environnement, 55290 Bure, France 20ERL, Institute of Nuclear and Radiological Science & Technology, Energy & Safety N.C.S.R. “Demokritos”, Attiki, Greece 21Institut National de l’Environnement Industriel et des Risques (INERIS), Verneuil-en-Halatte, France 22Meteorological Observatory Hohenpeissenberg, Hohenpeißenberg, German Weather Service, Germany 23Department of Atmospheric Sciences, University of Utah, Salt Lake City, UT 84112, USA 24Environmental Chemical Processes Laboratory (ECPL), University of Crete, Heraklion, Crete, 71003, Greece 25Institute of Chemical Technlogies and Analytics, TU Wien, Vienna, Austria 26CSIRO Oceans and Atmosphere, PMB1 Aspendale, VIC, Australia 27Global Atmosphere Watch Team, Innovative Meteorological Research Department, National Institute of Meteorological Sciences, Seogwipo-si, Jeju-do, Korea 28School of Earth and Environmental Sciences, Seoul National University, Seoul, Korea 29Division of Nuclear Physics, Department of Physics, Lund University, Lund, Sweden 30Atmospheric composition research, Finnish Meteorological Institute, Helsinki, Finland 31Svalbard Integrated Arctic Earth Observing System, Longyearbyen, Svalbard, Norway 32Department of Atmospheric Sciences, National Central University, Taoyuan, Taiwan 33Center for Environmental Monitoring Technology, National Central University, Taoyuan, Taiwan 34Institute of Atmospheric Sciences and Climate, National Research Council of Italy, Bologna, Italy 35Joint Research Centre (JRC), European Commission, Ispra, Italy 36Department of Environmental Science, University of Puerto Rico, Rio Piedras Campus, San Juan, Puerto Rico 37Observatoire des Sciences de l’Univers de La Réunion (OSUR), UMS3365, Saint-Denis de la Réunion, France 38Institute of Environmental Research & Sustainable Development, National Observatory of Athens, Palea Penteli, 15236, Greece 39Department of Aerosol Chemistry and Physics, Institute of Chemical Process Fundamentals, CAS, Prague, Czech Republic 40Laboratoire des Sciences du Climat et de l’Environnement, LSCE/IPSL, UMR 8212 CEA-CNRS-UVSQ, Université Paris-Saclay, Gif-sur-Yvette, France 41Laboratoire d’Aérologie, CNRS-Université de Toulouse, CNRS, UPS, Toulouse, France 42Environment and Climate Change Canada, Toronto, ON, Canada 43Sonnblick Observatory, ZAMG, 5020 Salzburg, Austria 44Department of Physics and Astronomy, Appalachian State University, Boone, NC, USA 45Atmospheric Sounding Station, El Arenosillo, Atmospheric Research and Instrumentation Branch, INTA, 21130, Mazagón, Huelva, Spain 46State Key Laboratory of Severe Weather & Key Laboratory of Atmospheric Chemistry of CMA, Chinese Academy of Meteorological Sciences, Beijing 100081, China 47Laboratoire de l’Atmosphère et des Cyclones (LACy), UMR8105, Université de la Réunion – CNRS – Météo-France, Saint-Denis de La Réunion, France 484S Company, 63000 Clermont-Ferrand, France 49Alfred-Wegener-Institut, Helmholtz-Zentrum für Polar-und Meeresforschung, 27570 Bremerhaven, Germany 50Univ. Grenoble-Alpes, CNRS, IRD, Grenoble-INP, IGE, 38000 Grenoble, France anow at: Department of Environmental Sciences, University of Basel, Basel, Switzerland

Funding Information:
The aerosol measurements at the Jungfraujoch were conducted with financial support from MeteoSwiss (GAW-CH aerosol monitoring programme) and from the European Union as well as the Swiss State Secretariat for Education, Research and Innovation (SERI) for the European Research Infrastructure for the observation of Aerosol, Clouds and Trace Gases (ACTRIS). The International Foundation High Altitude Research Station Jungfraujoch and Gornergrat (HFSJG) is mentioned for providing the research platform at the Jungfraujoch.

Funding Information:
VAV is grateful for various Swedish FORMAS, Swedish Research Council (VR) grants and the Magnus Bergvall and Märta och Erik Holmberg foundations and the Swedish EPA for making the research possible at the VAV site.

Funding Information:
Financial support. This research was supported by the European

Funding Information:
Sites PDM, PUY, GIF, CHC and RUN are partially operated with the support of CNRS-INSU under the long-term observation programme and the French Ministry for Research under the ACTRIS-FR national research infrastructure. PDM and GIF received specific support from the French Ministry of the Environment. ATMO Occitanie is mentioned for sampling operations at PDM. Measurements at SIRTA are hosted by CNRS and by the alternative energies and atomic energy commission (CEA) with additional contributions from the French Ministry of the Environment through its funding to the reference laboratory for air quality monitoring (LCSQA). PUY is grateful for support from ATMO Auvergne Rhône Alpes for sampling operations and the support from the personnel of the Observa-toire de Physique du Globe de Clermont-Ferrand (OPGC). The specific support of the Institut de Recherche et Développement (IRD) in France and the Universidad Mayor de San Andrés in Bolivia support operations at CHC operations.

Funding Information:
The aerosol measurements at Kosetice received funding from the European Union’s Horizon 2020 research and innovation programme under grant agreement no. 654109 and from the project for support of the national research infrastructure ACTRIS – participation of the Czech Republic (ACTRIS-CZ – LM2015037) supported by the Ministry of Education, Youth and Sports of CR within National Sustainability Program I (NPU I), grant agreement no. LO1415. The measurements were also supported by ERDF “ACTRIS-CZ RI” (no. CZ.02.1.01/0.0/0.0/16_013/0001315).

Funding Information:
At CMN, aerosol measurements were partially supported by the Italian Ministry of Research and Education.

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